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Abstract Multi-junction solar cells made by assembling semiconductor materials with different bandgap energies have hold the record conversion efficiencies for many years and are currently approaching 50%. Theoretical efficiency limits make use of optimum designs with the right lattice constant-bandgap energy combination, which requires a 1.0–1.15 eV material lattice-matched to GaAs/Ge. Nevertheless, the lack of suitable semiconductor materials is hindering the achievement of the predicted efficiencies, since the only candidates were up to now complex quaternary and quinary alloys with inherent epitaxial growth problems that degrade carrier dynamics. Here we show how the use of strain-balanced GaAsSb/GaAsN superlattices might solve this problem. We demonstrate that the spatial separation of Sb and N atoms avoids the ubiquitous growth problems and improves crystal quality. Moreover, these new structures allow for additional control of the effective bandgap through the period thickness and provide a type-II band alignment with long carrier lifetimes. All this leads to a strong enhancement of the external quantum efficiency under photovoltaic conditions with respect to bulk layers of equivalent thickness. Our results show that GaAsSb/GaAsN superlattices with short periods are the ideal (pseudo)material to be integrated in new GaAs/Ge-based multi-junction solar cells that could approach the theoretical efficiency limit.

Abstract As promising candidates for solar cell and photodetection applications in the range 1.0–1.16 eV, the growth of dilute nitride GaAsSbN alloys lattice matched to GaAs is studied. With this aim, we have taken advantage of the temperature gradient in the molecular beam epitaxy reactor to analyse the impact of temperature on the incorporation of Sb and N species according to the wafer radial composition gradients. The results from the combination of X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopies (EDS) show an opposite rate of incorporation between N and Sb as we move away from the centre of the wafer. A competitive behaviour between Sb and N in order to occupy the group-V position is observed that depends on the growth rate and the substrate temperature. The optical properties obtained by photoluminescence are discussed in the frame of the double-band anticrossing model. The growth conditions define two sets of different parameters for the energy level and the coupling interaction potential of N, which must be taken into account in the search for the optimum compositions 1–1.15-eV photonic applications.

A procedure to quantitatively analyse the relationship between the wetting layer (WL) and the quantum dots (QDs) as a whole in a statistical way is proposed. As we will show in the manuscript, it allows determining, not only the proportion of deposited InAs held in the WL, but also the average In content inside the QDs. First, the amount of InAs deposited is measured for calibration in three different WL structures without QDs by two methodologies: strain mappings in high-resolution transmission electron microscopy images and compositional mappings with ChemiSTEM x-ray energy spectrometry. The area under the average profiles obtained by both methodologies emerges as the best parameter to quantify the amount of InAs in the WL, in agreement with high-resolution x-ray diffraction results. Second, the effect of three different GaAs capping layer (CL) growth rates on the decomposition of the QDs is evaluated. The CL growth rate has a strong influence on the QD volume as well as the WL characteristics. Slower CL growth rates produce an In enrichment of the WL if compared to faster ones, together with a diminution of the QD height. In addition, assuming that the QD density does not change with the different CL growth rates, an estimation of the average In content inside the QDs is given. The high Ga/In intermixing during the decomposition of buried QDs does not only trigger a reduction of the QD height, but above all, a higher impoverishment of the In content inside the QDs, therefore modifying the two most important parameters that determine the optical properties of these structures. [ABSTRACT FROM AUTHOR]

The effect of the capping process on the morphology of InAs/GaAs quantum dots (QDs) by using different GaAs-based capping layers (CLs), ranging from strain reduction layers to strain compensating layers, has been studied by transmission microscopic techniques. For this, we have measured simultaneously the height and diameter in buried and uncapped QDs covering populations of hundreds of QDs that are statistically reliable. First, the uncapped QD population evolves in all cases from a pyramidal shape into a more homogenous distribution of buried QDs with a spherical-dome shape, despite the different mechanisms implicated in the QD capping. Second, the shape of the buried QDs depends only on the final QD size, where the radius of curvature is function of the base diameter independently of the CL composition and growth conditions. An asymmetric evolution of the QDs’ morphology takes place, in which the QD height and base diameter are modified in the amount required to adopt a similar stable shape characterized by a averaged aspect ratio of 0.21. Our results contradict the traditional model of QD material redistribution from the apex to the base and point to a different universal behavior of the overgrowth processes in self-organized InAs QDs. [ABSTRACT FROM AUTHOR]

Type II emission optoelectronic devices using GaAsSb strain reduction layers (SRL) over InAs quantum dots (QDs) have aroused great interest. Recent studies have demonstrated an extraordinary increase in photoluminescence (PL) intensity maintaining type II emission after a rapid thermal anneal (RTA), but with an undesirable blueshift. In this work, we have characterized the effect of RTA on InAs/GaAs QDs embedded in a SRL of GaAsSb by transmission electron microscopy (TEM) and finite element simulations. We find that annealing alters both the distribution of Sb in the SRL as well as the exchange of cations (In and Ga) between the QDs and the SRL. First, annealing causes modifications in the capping layer, reducing its thickness but maintaining the maximum Sb content and improving its homogeneity. In addition, the formation of Sb-rich clusters with loop dislocations is noticed, which seems not to be an impediment for an increased PL intensity. Second, RTA produces flatter QDs with larger base diameter and induces a more homogeneous QD height distribution. The Sb is accumulated over the QDs and the RTA enlarges the Sb-rich region, but the Sb contents are very similar. This fact leaves the type II alignment without major changes. Atomic-scale strain analysis of the nanostructures reveal a strong intermixing of In/Ga between the QDs and the capping layer, which is the main responsible mechanism of the PL blueshift. The improvement of the crystalline quality of the capping layer together with higher homogeneity QD sizes could be the origin of the enhancement of the PL emission. [ABSTRACT FROM AUTHOR]

This work presents a comprehensive optical characterization of Zn1−xMgxO thin films grown by spray pyrolysis (SP). Absorption measurements show the high potential of this technique to tune the bandgap from 3.30 to 4.11 eV by changing the Mg acetate content in the precursor solution, leading to a change of the Mg-content ranging from 0 up to 35%, as measured by transmission electron microscopy-energy dispersive x-ray spectroscopy. The optical emission of the films obtained by cathodoluminescence and photoluminescence spectroscopy shows a blue shift of the peak position from 3.26 to 3.89 eV with increasing Mg incorporation, with a clear excitonic contribution even at high Mg contents. The linewidth broadening of the absorption and emission spectra as well as the magnitude of the observed Stokes shift are found to significantly increase with the Mg content. This is shown to be related to both potential fluctuations induced by pure statistical alloy disorder and the presence of a tail of band states, the latter dominating for medium Mg contents. Finally, metal–semiconductor–metal photodiodes were fabricated showing a high sensitivity and a blue shift in the cut-off energy from 3.32 to 4.02 eV, i.e., down to 308 nm. The photodiodes present large UV/dark contrast ratios (102 − 107), indicating the viability of SP as a growth technique to fabricate low cost (Zn, Mg)O-based UV photodetectors reaching short wavelengths. [ABSTRACT FROM AUTHOR]

A detailed analysis of the impact of illumination on the electrical response of In0.5Ga0.5As surface nanostructures is carried out as a function of different relative humidity conditions. The importance of the surface-to-volume ratio for sensing applications is once more highlighted. From dark-to-photo conditions, the sheet resistance (SR) of a three-dimensional In0.5Ga0.5As nanostructure decays two orders of magnitude compared with that of a two-dimensional nanostructure. The electrical response is found to be vulnerable to the energy of the incident light and the external conditions. Illuminating with high energy light translates into an SR reduction of one order of magnitude under humid atmospheres, whereas it remains nearly unchanged under dry environments. Conversely, lighting with energy below the bulk energy bandgap, shows a negligible effect on the electrical properties regardless the local moisture. Both illumination and humidity are therefore needed for sensing. Photoexcited carriers can only contribute to conductivity if surface states are inactive due to water physisorption. The strong dependence of the electrical response on the environment makes these nanostructures very suitable for the development of highly sensitive and efficient sensing devices. [ABSTRACT FROM AUTHOR]

The use of Sb during the capping process of quantum dots (QDs) to tune the emission wavelength has been investigated by means of cross-sectional scanning tunneling microscopy (X-STM), photoluminescence (PL) measurements and atomic force microscopy. It is found that a capping layer of GaAsSb reduces InAs/GaAs QD decomposition during capping due to the smaller lattice mismatch with the QD and due to the surfactant effect of Sb. An Sb content of 14% in the GaAsSb layer has been found to be sufficient to eliminate the QD decomposition completely and improve the PL properties. Further increase in the Sb content causes a degradation of the PL properties. Reduction of the QD decomposition has also been achieved by soaking the QDs with Sb before the capping. Furthermore, it is shown that the segregation of In and of Sb in the Ga and the As sublattices respectively are two independent processes. Similar investigations to the use of Sb to tune InAs/InP (311B) QDs are reported. Also in this case, the use of Sb, either in the form of elemental Sb or as a GaAsSb alloy, has resulted in elimination of QD decomposition. [ABSTRACT FROM AUTHOR]

The growth mechanism of stacked InAs/InP(001) quantum wires (QWRs) is studied by combining an atomic-scale cross-sectional scanning tunnelling microscopy analysis with in situ and in real-time stress measurements along the [110] direction (sensitive to stress relaxation during QWR formation). QWRs in stacked layers grow by a non-Stranski-Krastanov (SK) process which involves the production of extra InAs by strain-enhanced As/P exchange and a strong strain driven mass transport. Despite the different growth mechanism of the QWR between the first and following layers of the stack, the QWRs maintain on average the same shape and composition in all the layers of the stack, revealing the high stability of this QWR configuration. [ABSTRACT FROM AUTHOR]